CN106977828A - A kind of fiber reinforcement sebific duct inside and outside glue material and preparation method thereof and sebific duct - Google Patents

A kind of fiber reinforcement sebific duct inside and outside glue material and preparation method thereof and sebific duct Download PDF

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CN106977828A
CN106977828A CN201710240004.0A CN201710240004A CN106977828A CN 106977828 A CN106977828 A CN 106977828A CN 201710240004 A CN201710240004 A CN 201710240004A CN 106977828 A CN106977828 A CN 106977828A
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parts
sebific duct
pur
rubber
fiber reinforcement
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畅延明
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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/26Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers modified by chemical after-treatment
    • C08L23/28Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers modified by chemical after-treatment by reaction with halogens or compounds containing halogen
    • C08L23/286Chlorinated polyethylene
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F16ENGINEERING ELEMENTS AND UNITS; GENERAL MEASURES FOR PRODUCING AND MAINTAINING EFFECTIVE FUNCTIONING OF MACHINES OR INSTALLATIONS; THERMAL INSULATION IN GENERAL
    • F16LPIPES; JOINTS OR FITTINGS FOR PIPES; SUPPORTS FOR PIPES, CABLES OR PROTECTIVE TUBING; MEANS FOR THERMAL INSULATION IN GENERAL
    • F16L11/00Hoses, i.e. flexible pipes
    • F16L11/04Hoses, i.e. flexible pipes made of rubber or flexible plastics
    • F16L11/08Hoses, i.e. flexible pipes made of rubber or flexible plastics with reinforcements embedded in the wall
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2203/00Applications
    • C08L2203/18Applications used for pipes
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/03Polymer mixtures characterised by other features containing three or more polymers in a blend
    • C08L2205/035Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/04Polymer mixtures characterised by other features containing interpenetrating networks
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/14Polymer mixtures characterised by other features containing polymeric additives characterised by shape
    • C08L2205/16Fibres; Fibrils
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2207/00Properties characterising the ingredient of the composition
    • C08L2207/04Thermoplastic elastomer
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2312/00Crosslinking

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • General Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Laminated Bodies (AREA)

Abstract

The invention discloses a kind of fiber reinforcement sebific duct inside and outside glue material and its preparation and sebific duct, it is related to synthetic rubber field, fiber reinforcement is polyester fiber, and material feedstock composition includes:Chlorinated polyethylene rubber, PUR and vulcanization accelerator, the PUR are thermoplastic elastomer (TPE).By PUR as inside and outside glue and the bridge of fiber reinforcement, significantly increase the intensity and toughness of skeleton sebific duct, while improving sebific duct prevents old ability and peel strength.

Description

A kind of fiber reinforcement sebific duct inside and outside glue material and preparation method thereof and sebific duct
Technical field
The present invention relates to synthetic rubber field, and in particular to a kind of fiber reinforcement sebific duct with inside and outside glue material and its sebific duct and Preparation method.
Background technology
Chlorinated polyethylene rubber (abbreviation CM rubber) is through randomly chlorinated one kind by high density polyethylene (HDPE) (HDPE) Tartan.It is the terpolymer of ethene, vinyl chloride and 1,2- vinylidene chloride polymerizations segment composition.Point of CM rubber Sub- main chain is made up of carbon-to-carbon singly-bound, is a kind of chloride rubber of saturation.The molecular structure feature determines that it has well resistance to Hot, ozone resistance, resistance to weather, oil resistivity, chemical proofing, lower temperature resistance, resistance to bacterium and microbes and electrically Many excellent performances such as performance and anti-flammability;And CM rubber wide material sources, it is cheap, electric wire, cable are can apply to, Offset plate, pressing and steel wire high-pressure rubber pipe glue etc..
But, CM rubber applications field product structure is mainly pure glue or metallic framework sebific duct product.Pure glue sebific duct is born Hypotony uses the cobalt salt adhesive that is used in narrow range, metal skeleton product CM rubber and metal sulfuration adhesion good and not shadow CM vulcanization is rung, but cobalt salt adhesive is unable to bonded polyester material, also, conventional curing agent is bonded in rubber and existing fiber Easily occur oxidative decomposition in system and fail, make sebific duct intensity too low.
The content of the invention
For above-mentioned problem of the prior art, it is an object of the invention to provide glue material inside and outside a kind of fiber reinforcement sebific duct Material and preparation method thereof and sebific duct, by PUR as inside and outside glue and the bridge of fiber reinforcement, make the intensity of skeleton sebific duct Significantly increased with toughness, while improving sebific duct prevents old ability and peel strength.
A kind of fiber reinforcement sebific duct is polyester fiber with inside and outside glue material, fiber reinforcement, and material feedstock composition includes:Chlorination Polyethylene rubber, PUR and vulcanization accelerator, the PUR are thermoplastic elastomer (TPE).Polyester fiber is specially organic binary Acid and the polyester of dihydric alcohol polycondensation are through the synthetic fibers obtained by spinning.
The thermoplastic elastomer (TPE) is preferably ethylene ethyl acrylate copolymer, and/or
The thermoplastic elastomer (TPE) is added in mix stage.
It is linear that the present invention significantly inhibits haloflex singly-bound main chain in the high-temperature mixing stage using PUR.Specifically, It utilizes carboxyl itself and molecular polarity, and producing stronger dipole moment with CM rubber halogen group is acted on, and it is enhanced indirectly with gathering Hydrogen bond between ester fiber, promotes polyester fiber and the follow-up vulcanization crosslinking of CM rubber, the side base of polyester fiber is participated in inside and outside glue Interpenetrating networks reaction so that using intermolecular force → vulcanization crosslinking chemical bond → network interpenetrating main chain, progressively it is progressive simultaneously Synergistic a variety of effects, significantly improve the tensile strength of sebific duct with peeling off ageing resistace.
It is preferred that, the vulcanization accelerator is thiadiazoles and its derivative vulcanizing system accelerator, the vulcanization accelerator Further preferably aliphatic amide and secondary aliphatic amine condensation product.Further, the vulcanization accelerator is preferably ACCEL-BF.
It is preferred that, above-mentioned material raw material composition and its weight proportion include:100 parts of chlorinated polyethylene rubber, PUR 8- 15 parts, MgO6-12 parts, wax class prevent old lubricant 5-6 parts, 7-8 parts of activating agent, 84-94 parts of rubber reinforcing filler, phthalic acid two 5-6 parts of 35-45 parts of monooctyl ester (abbreviation DOP), 10-14 parts of colouring agent, 7-13 parts of resin reinforcing agent and vulcanization accelerator.
A kind of preparation method of above-mentioned material is further provided for, preparation process includes:
1. weighed according to parts by weight:100 parts of chlorinated polyethylene rubber, 10-15 parts of PUR and activity MgO10-12 parts, wax Class prevents old lubricant 5-6 parts, 7-8 parts of activating agent, 11-13 parts of colouring agent, 7~11 parts of input mixer mixings of resin reinforcing agent 0.5-2min,
2. by 85~94 parts of rubber reinforcing filler, 7~13 parts of input banburyings of 35~45 parts of dioctyl phthalate and resin Machine, 100-130 DEG C of mixing temperature kneads 5-8min, acts the discharge that sticks together,
3. through 50-300 mesh filter screens filter after, on a mill add 5-6 part of vulcanization accelerator, by repeatedly it is thin lead to after, Bottom sheet storage is stand-by.
It is preferred that, PUR is 15 parts by weight, and resin reinforcing agent is 7 parts, and rubber reinforcing filler is 94 parts, phthalic acid two Pungent fat is 43 parts.
Further provide for mesolow sebific duct prepared by a kind of above-mentioned material or above-mentioned preparation method resulting materials.
It is preferred that, above-mentioned mesolow sebific duct is extruded, sulphur using the material and polyester fiber establishment skeleton by inside and outside glue It is prepared by chemical conversion type.
The resultant effect that the present invention is brought includes:
The present invention adds PUR in mixing, is combined using its chemical constitution with CM rubber and polyester fiber, is ensureing On the premise of tensile strength is excellent, the antitorque of this kind of material and gained polyester fiber skeleton mesolow sebific duct is significantly improved Anti-aging and antistripping resistanee to rupture.
Embodiment
Explanation is further explained to the present invention with reference to specific embodiment and detection data, it should be appreciated that the present invention Scope not limited to this.
Material properties test
This test is carried out using Kunshan Jing Xintong Electronic Science and Technology Co., Ltd.s JX-6010 model rubber tensiles strength tester Detection.Sample is measured with reference to DB37/T 2263-2012 and GB16491-2008 standard and instrumentation flow.Each material Expect that the performance test results are as shown in table 1.
Embodiment 1
A kind of fiber reinforcement sebific duct is PET polyester fibers with inside and outside glue material, fiber reinforcement, and material feedstock composition includes: Chlorinated polyethylene rubber, PUR and vulcanization accelerator, the PUR are thermoplastic elastomer (TPE).
The thermoplastic elastomer (TPE) is ethylene acrylic acid co polymer, the specific EAA378 using E.I.Du Pont Company.
The vulcanization accelerator is thiadiazoles and its derivative vulcanizing system accelerator, and the vulcanization accelerator contains fat Race's acid amides and secondary aliphatic amine condensation product.Further, the vulcanization accelerator is specially ACCEL-BF.
Above-mentioned material raw material is constituted and its weight proportion includes:Chlorinated polyethylene rubber 100kg, PUR 10kg, activity MgO10kg, wax class prevent old lubricant 5.5kg, activating agent polyethylene glycol 7.5kg, rubber reinforcing filler white carbon 85kg, DOP35kg, Colouring agent 12kg, resin reinforcing agent 13kg and vulcanization accelerator 5.1kg.
A kind of preparation method of above-mentioned material is further provided for, preparation process includes:
1. weighed according to weight kg:Chlorinated polyethylene rubber 100kg, PUR 10kg and activity MgO10kg, wax class are anti-old Lubricant 5.5kg, activating agent 7.5kg, colouring agent 12kg, resin reinforcing agent 13kg input mixer mixing 1min,
2. rubber reinforcing filler 85kg, dioctyl phthalate 35kg and coumarone indene resin 10kg are put into banbury, it is close 110 DEG C of temperature is refined, 6min is kneaded, the discharge that sticks together is acted,
3. after being filtered through 100 mesh filter screens, vulcanization accelerator 5.1kg is added on a mill, after thin 3 times lead to, bottom sheet Storage is stand-by.
The mesolow sebific duct for further preparing above-mentioned material or above-mentioned preparation method resulting materials:
Above-mentioned mesolow sebific duct is extruded, sulfidization molding using the material and polyester fiber establishment skeleton by inside and outside glue Prepare.
Embodiment 2
A kind of fiber reinforcement sebific duct is PBT polyester fiber with inside and outside glue material, fiber reinforcement, and material feedstock composition includes: Chlorinated polyethylene rubber, PUR and vulcanization accelerator, the PUR are thermoplastic elastomer (TPE).
The thermoplastic elastomer (TPE) is ethylene acrylic acid co polymer, the specific EAA378 using E.I.Du Pont Company.
The vulcanization accelerator is thiadiazoles and its derivative vulcanizing system accelerator, and the vulcanization accelerator contains fat Race's acid amides and secondary aliphatic amine condensation product.Further, the vulcanization accelerator is specially ACCEL-BF.
Above-mentioned material raw material is constituted and its weight proportion includes:Chlorinated polyethylene rubber 100kg, PUR 10kg, activity MgO10kg, wax class prevent old lubricant 5.5kg, the coupling agent 7.5kg of activating agent silicon 69, the strong prestige powder 94kg of rubber reinforcing filler, DOP45kg, colouring agent 12kg, resin reinforcing agent 11kg and vulcanization accelerator 5.1kg.
A kind of preparation method of above-mentioned material is further provided for, preparation process includes:
1. weighed according to weight kg:Chlorinated polyethylene rubber 100kg, PUR 10kg and activity MgO10kg, wax class are anti-old Lubricant 5.5kg, activating agent 7.5kg, colouring agent 12kg, resin reinforcing agent 11kg input mixer mixing 1min,
2. rubber reinforcing filler 94kg, dioctyl phthalate 45kg and coumarone indene resin 12kg are put into banbury, it is close 110 DEG C of temperature is refined, 6min is kneaded, the discharge that sticks together is acted,
3. after being filtered through 100 mesh filter screens, vulcanization accelerator 5.1kg is added on a mill, after thin 3 times lead to, bottom sheet Storage is stand-by.
The mesolow sebific duct for further preparing above-mentioned material or above-mentioned preparation method resulting materials:
Above-mentioned mesolow sebific duct is extruded, sulfidization molding using the material and polyester fiber establishment skeleton by inside and outside glue Prepare.
Embodiment 3
A kind of fiber reinforcement sebific duct is polyarylate fiber with inside and outside glue material, fiber reinforcement, and material feedstock composition includes:Chlorine Change polyethylene rubber, PUR and vulcanization accelerator, the PUR is thermoplastic elastomer (TPE).
The thermoplastic elastomer (TPE) is ethylene acrylic acid co polymer, the specific EAA378 using E.I.Du Pont Company.
The vulcanization accelerator is thiadiazoles and its derivative vulcanizing system accelerator, and the vulcanization accelerator contains fat Race's acid amides and secondary aliphatic amine condensation product.Further, the vulcanization accelerator is specially ACCEL-BF.
Above-mentioned material raw material is constituted and its weight proportion includes:Chlorinated polyethylene rubber 100kg, PUR 15kg, activity MgO12kg, wax class prevent old lubricant 5.5kg, activating agent polyethylene glycol 7.5kg, rubber reinforcing filler white carbon 94kg, DOP43kg, Colouring agent 12kg, resin reinforcing agent 7kg and vulcanization accelerator 5.1kg.
A kind of preparation method of above-mentioned material is further provided for, preparation process includes:
1. weighed according to weight kg:Chlorinated polyethylene rubber 100kg, PUR 15kg and activity MgO12kg, wax class are anti-old Lubricant 5.5kg, activating agent polyethylene glycol 7.5kg, colouring agent 12kg, resin reinforcing agent 7kg input mixer mixing 1min,
2. rubber reinforcing filler 94kg, dioctyl phthalate 43kg and coumarone indene resin 8kg are put into banbury, banburying 110 DEG C of temperature, kneads 6min, acts the discharge that sticks together,
3. after being filtered through 100 mesh filter screens, vulcanization accelerator 5.1kg is added on a mill, after thin 3 times lead to, bottom sheet Storage is stand-by.
The mesolow sebific duct for further preparing above-mentioned material or above-mentioned preparation method resulting materials:
Above-mentioned mesolow sebific duct is extruded, sulfidization molding using the material and polyester fiber establishment skeleton by inside and outside glue Prepare.
Comparative example 1
This comparative example is implemented using glue material inside and outside embodiment 1 and mesolow sebific duct preparation method, and difference exists In vulcanizing system is changed to adopt by PUR component of the present embodiment in inside and outside glue material formula without thermoplastic elastomer (TPE) With m- first-lean type system, Inner glue, polyester fiber skeleton and outer glue three are vulcanized and bonded.Specifically, in silica-hexa-resorcinol, first Aldehyde donor be hexamethylenetetramine, be resorcinol, white carbon is hydrated SiO 2.Silica-hexa-resorcinol system is in sulfidation In, resorcinol directly can not react with CM rubber halogen groups, and interference is giving group cross-linking reaction just with formaldehyde Often carry out, and promote polyester fiber to hydrolyze, skeleton accelerated ageing.Visible adds lean type system rubber vulcanization insufficient in table 1, hence it is evident that Owe sulphur.
Comparative example 2
This comparative example is implemented using glue material inside and outside embodiment 1 and mesolow sebific duct preparation method, and difference exists In PUR component of the present embodiment in inside and outside glue material formula without thermoplastic elastomer (TPE), vulcanizing system is still used Thiadiazole Curing System and corresponding vulcanization accelerator, are carried out Inner glue, polyester fiber skeleton and outer glue three using crosslinking Vulcanize and bond.Specifically, in sulfidation, although the CM rubber in inside and outside glue can normally vulcanize, resist with certain Tensile strength.But fiber reinforcement can not effectively be bonded, only inner outer glue vulcanizes the physics to be formed inclusion power and fixed.Turning round Pull with stripping process, fiber reinforcement promotes inside and outside glue separation, triplicity intensity is substantially reduced.
The material sebific duct performance detection of table 1
Numbering Tensile strength Elongation Setafter break Internal layer peel strength Outer layer peel strength
Embodiment 1 5.5MPa 233.3% 29.3% 23N/25mm 31N/25mm
Embodiment 2 7.5MPa 440% 68% 32.4N/25mm 41.5N/25mm
Embodiment 3 8.5MPa 520% 48% 45.2N/25mm 56.7N/25mm
Comparative example 1 3.8MPa 650% 220% 10M/25mm 15N/25mm
Comparative example 2 5.0MPa 200.6% 119.3% 15N/25mm 14N/25mm
Although the present invention has been described in detail, it will be understood by those skilled in the art that in spirit and scope of the invention Modification will be apparent.However, it should be understood that each side of the invention recorded, different embodiments Each several part and the various features enumerated can be combined or all or part of exchange.In each above-mentioned embodiment, that A little embodiments with reference to another embodiment can be combined suitably with other embodiment, and this is by by this area skill Art personnel are to understand.In addition, it will be understood to those of skill in the art that description above is only the mode of example, not purport In the limitation present invention.

Claims (8)

1. glue material inside and outside a kind of fiber reinforcement sebific duct, it is characterised in that fiber reinforcement is polyester fiber, material feedstock composition Including:Chlorinated polyethylene rubber, PUR and vulcanization accelerator, the PUR are thermoplastic elastomer (TPE).
2. material according to claim 1, it is characterised in that the thermoplastic elastomer (TPE) is ethylene ethyl acrylate copolymerization Thing, and/or the thermoplastic elastomer (TPE) are added in mix stage.
3. material according to claim 1 or 2, it is characterised in that the vulcanization accelerator is thiadiazoles and its derivative Vulcanizing system accelerator, preferably comprises the condensation product of aliphatic amide and secondary aliphatic amine.
4. material according to claim 3, it is characterised in that material feedstock is constituted and its weight proportion includes:Chlorination gathers 100 parts of ethylene rubber, 8-15 parts of PUR, MgO6-12 parts, wax class prevent old lubricant 5-6 parts, 7-8 parts of activating agent, reinforcing rubber 84-94 parts of agent, 35-45 parts of dioctyl phthalate, 10-14 parts of colouring agent, 7-13 parts of resin reinforcing agent and vulcanization accelerator 5-6 parts.
5. a kind of preparation method of the material as any one of claim 1-4, it is characterised in that preparation process includes:
1. weighed according to parts by weight:MgO10-12 parts of 100 parts of chlorinated polyethylene rubber, 10-15 parts of PUR and activity, wax class are prevented Old lubricant 5-6 parts, 7-8 parts of activating agent, 11-13 parts of colouring agent, 7-11 parts of input mixer mixing 0.5- of resin reinforcing agent 2min,
2. by 85~94 parts of rubber reinforcing filler, 7-13 parts of input banburies of 35-45 parts of dioctyl phthalate and resin, banburying 100-130 DEG C of temperature, kneads 5-8min, acts the discharge that sticks together,
3. through 50-300 mesh filter screens filter after, on a mill add 5-6 part of vulcanization accelerator, by repeatedly it is thin lead to after, bottom sheet Storage is stand-by.
6. preparation method according to claim 5, it is characterised in that PUR is 15 parts, resin reinforcing agent is 7 parts, rubber Glue reinforcing agent is 94 parts, and o-phthalic acid dibutyl ester is 43 parts.
7. one kind material or preparation method institute as any one of claim 5-6 as any one of claim 1-4 Obtain fiber reinforcement mesolow sebific duct prepared by material.
8. fiber reinforcement mesolow sebific duct according to claim 7, it is characterised in that use the material and polyester fiber Skeleton is woven, is extruded by inside and outside glue, be prepared by sulfidization molding.
CN201710240004.0A 2017-04-13 2017-04-13 A kind of fiber reinforcement sebific duct inside and outside glue material and preparation method thereof and sebific duct Pending CN106977828A (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1351236A (en) * 2001-12-07 2002-05-29 甘国工 Stretch-orientated cross-linked polymer pipe
CN105299341A (en) * 2015-12-04 2016-02-03 沈阳赛亚橡胶制品有限公司 Vehicle fuel hose resistant to high pressure and low in permeability
CN106147051A (en) * 2016-06-30 2016-11-23 五行科技股份有限公司 A kind of flexible pipe and manufacture method thereof

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1351236A (en) * 2001-12-07 2002-05-29 甘国工 Stretch-orientated cross-linked polymer pipe
CN105299341A (en) * 2015-12-04 2016-02-03 沈阳赛亚橡胶制品有限公司 Vehicle fuel hose resistant to high pressure and low in permeability
CN106147051A (en) * 2016-06-30 2016-11-23 五行科技股份有限公司 A kind of flexible pipe and manufacture method thereof

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
中国消防协会 编: "《灭火救援员.初级技能》", 31 December 2013, 中国科学技术出版社 *

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